First data on technetium-99 content in the ecosystem of the Yenisei River

The content of a long-lived technogenic radionuclide ⁹⁹Tc in the Yenisei within the territory of radioactive effluents of the Rosatom mining chemical combine (MCC) has been studied. In 2008–2009 the maximal ⁹⁹Tc content in water was registered near the dumping site of the MCC and came to 33 mBq/l. According to analysis of filtered water samples, technetium in the Yenisei water is presented as pertechnetate ion (TcO₄). When moving away from the MCC downstream, the ⁹⁹Tc content in water is decreased, which is caused both by dilution of waste water and by ⁹⁹Tc accumulation by aquatic plants. The ⁹⁹Tc content in the biomass of the aquatic plant Potamogeton lucens came to 82¹⁵ Bq/kg, and the concentration factor (CF) to 8200, which is three times more than the maximal values of the CF of ⁹⁹Tc by the plants in laboratory conditions (2700).     

Uranium isotopes as a tracer of sources of dissolved solutes in the Han River,South Korea

The uranium (U) content and ²³⁴U/²³⁸U activity ratio were determined for water samples collected from Korea's Han River in spring, summer, and winter 2006 to provide data that might constrain the origin of U isotope fractionation in river water and the link between U isotope systematics in river waters and the lithological nature of the corresponding bedrock. The large difference in the major dissolved loads between the two major branches of the Han River, the North Han River (NHR) and South Han River (SHR), is reflected in the contrasting U content and ²³⁴U/²³⁸U activity ratio between the tributaries: low U content (0.08–0.75 nM; average, 0.34 nM) and small ²³⁴U/²³⁸U activity ratio (1.03–1.22; average, 1.09) in the NHR; and high U content (0.65–1.98 nM; average, 1.44 nM) and large ²³⁴U/²³⁸U activity ratio (1.05–1.45; average, 1.24) in the SHR. The large spatial differences in U content and ²³⁴U/²³⁸U activity ratio are closely related to both lithological differences between the two tributaries and groundwater input. The low U content and small ²³⁴U/²³⁸U activity ratio in the NHR arise mainly from a combination of surface and meteoric weathering of the dominant silicate rocks in this branch and congruent dissolution of already weathered (secular equilibrium) materials. In contrast, the high U content and large ²³⁴U/²³⁸U activity ratio in the SHR are ascribed to the dissolution of carbonates and black shales along with significant inputs of deep groundwater.     

Dissolved Uranium and 234U/238U in the Yamuna and the Chambal Rivers, India

Dissolved uranium concentration and ²³⁴U/²³⁸U activity ratio have been measured in two distinctly different Indian drainage systems: the Yamuna headwaters in the Himalaya and the Chambal river system in the plains to study the weathering and mobility of uranium in these watersheds. The dissolved uranium in the Chambal river system ranges from 0.2 to 1.74 μg L⁻¹ during September (tail end of monsoon), whereas in the Yamuna river system, its concentration varies from 0.1 to 3.18 μg L⁻¹ during October (post-monsoon) and from 0.09 to 3.61 μg L⁻¹ in June (summer). In the Yamuna main stream, uranium is highest at its source and decreases steadily along its course, from 3.18 μg L⁻¹ at Hanuman Chatti to 0.67 μg L⁻¹ at Batamandi, at the base of the Himalaya. This decrease results mainly from mixing of the Yamuna mainstream with its tributaries, which are lower in uranium. The high concentration of uranium at Hanuman Chatti is derived from weathering of the Higher Himalayan Crystalline series (HHC) and associated accessary minerals, which may include uranium-mineralised zones. The ²³⁴U/²³⁸U activity ratios in the samples from the Chambal watershed are in the range of 1.15±0.05 to 1.67±0.04; whereas in the Yamuna the ratios vary from 0.95±0.03 to 1.56±0.07, during post-monsoon and from 0.98±0.01 to 1.30±0.03, during summer. The relatively high ²³⁴U/²³⁸U activity ratios in the Yamuna system are in its tributaries from the lower reaches viz., the Amlawa, Aglar, Bata, Tons and the Giri. It is estimated that ~9×10³ and ~12 × 10³ kg of dissolved uranium are transported annually from the Yamuna at Batamandi and the Chambal at Udi, respectively. This corresponds to uranium weathering rates of 0.9 and 0.09 kg U km⁻² y⁻¹ in the basins of the Yamuna and the Chambal headwaters. This study confirms that uranium weathering rate in the Himalaya is far in excess (by about an order of magnitude) of the global average value of ~0.08 kg U km⁻² y⁻¹.     

Geo-chemical Behavior of Uranium in the Sambhar Salt Lake, Rajasthan (India): Implications to "Source" of Salt and Uranium "Sink"

Among several salt lakes in the Thar Desert of western India, the Sambhar is the largest lake producing about 2 × 10⁵ tons of salt (NaCl) annually. The “lake system” (lake waters, inflowing river waters, and sub-surface brines) provides a unique setting to study the geo-chemical behavior of uranium isotopes (²³⁸U, ²³⁴U) in conjunction with the evolution of brines over the annual wetting and evaporation cycles. The concentration of ²³⁸U and the total dissolved solids (TDS) in lake water increase from ~8 μg L⁻¹ and ~8 g L⁻¹ in monsoon to ~1,400 μg L⁻¹ and 370 g L⁻¹, respectively, during summer time. The U/TDS ratio (~1 μg g⁻¹ salt) and the ²³⁴U/²³⁸U activity ratio (1.65 ± 0.05), however, remain almost unchanged throughout the year, except when U/TDS ratio approaches to 3.8 at/or beyond halite crystallization. These observations suggest that uranium behaves conservatively in the lake waters during the annual cycle of evaporation. Also, uranium and salt content (TDS) are intimately coupled, which has been used to infer the origin and source of salt in the lake basin. Furthermore, near uniform ratios in evaporating lake waters, when compared to the ratio in seawater (~0.1 μg g⁻¹ salt and 1.14 ± 0.02, respectively), imply that aeolian transport of marine salts is unlikely to be significant source of salt to the lake in the present-day hydrologic conditions. This inference is further consistent with the chemical composition of wet-precipitation occurring in and around the Sambhar lake. The seasonal streams feeding the lake and groundwaters (within the lake’s periphery) have distinctly different ratios of U/TDS (2–69 μg g⁻¹ salt) and ²³⁴U/²³⁸U (1.15–2.26) compared to those in the lake. The average U/TDS ratio of ~1 μg g⁻¹ salt in lake waters and ~19 μg g⁻¹ salt in river waters suggest dilution of the uranium content by the recycled salt and/or removal processes presently operating in the lake during the extraction of salt for commercial use. Based on mass-balance calculations, a conservative estimate of "uranium sink" (in the form of bittern crust) accounts for ~5 tons year⁻¹ from the lake basin, an estimate similar to its input flux from rivers, i.e., 4.4 tons year⁻¹.     

Isotope hydrology of the Chalk River Laboratories site,Ontario, Canada

This paper presents results of hydrochemical and isotopic analyses of groundwater (fracture water) and porewater, and physical property and water content measurements of bedrock core at the Chalk River Laboratories (CRL) site in Ontario. Density and water contents were determined and water-loss porosity values were calculated for core samples. Average and standard deviations of density and water-loss porosity of 50 core samples from four boreholes are 2.73 ± 12 g/cc and 1.32 ± 1.24 percent. Respective median values are 2.68 and 0.83 indicating a positive skewness in the distributions. Groundwater samples from four deep boreholes were analyzed for strontium (⁸⁷Sr/⁸⁶Sr) and uranium (²³⁴U/²³⁸U) isotope ratios. Oxygen and hydrogen isotope analyses and selected solute concentrations determined by CRL are included for comparison. Groundwater from borehole CRG-1 in a zone between approximately +60 and −240 m elevation is relatively depleted in δ¹⁸O and δ²H perhaps reflecting a slug of water recharged during colder climatic conditions. Porewater was extracted from core samples by centrifugation and analyzed for major dissolved ions and for strontium and uranium isotopes. On average, the extracted water contains 15 times larger concentration of solutes than the groundwater. ²³⁴U/²³⁸U and correlation of ⁸⁷Sr/⁸⁶Sr with Rb/Sr values indicate that the porewater may be substantially older than the groundwater. Results of this study show that the Precambrian gneisses at Chalk River are similar in physical properties and hydrochemical aspects to crystalline rocks being considered for the construction of nuclear waste repositories in other regions.     

粤北长江铀矿田花岗岩独居石U-Pb同位素定年及其地质意义

长江铀矿田位于诸广山复式岩体中南部,是典型的花岗岩型铀矿田.前人采用锆石U-Pb定年方法对赋矿花岗岩进行了年代学研究,但由于全岩和锆石铀含量较高,锆石往往发生了蜕晶化,可能导致锆石U-Pb定年数据散乱,影响锆石U-Pb年龄的可靠性.独居石是花岗岩中广泛存在的含铀副矿物,铀和钍含量均较高,可达10000×10-6,普通铅...     

Behavior of Uranium in the Yellow River Plume (Yellow River Estuary)

The Yellow River (Huanghe) is the second largest river in China and is known for its high turbidity. It also has remarkably high levels of dissolved uranium (U) concentrations (up to 38 nmol 1^-1). To examine the mixing behavior of dissolved U between river water and seawater, surface water samples were collected along a salinity gradient from the Yellow River plume during September 2004 and were measured for dissolved U concentration,²³⁴U:²³⁸U activity ratio, phosphate (PO₄ ^3–), and suspended particulate matter. Laboratory experiments were also conducted to simulate the mixing process in the Yellow River plume using unfiltered Yellow River water and filtered seawater. The results showed a nonconservative behavior for dissolved U at salinities < 20 with an addition of U to the plume waters estimated at about 1.4 X 10⁵ mol yr^–1. A similarity between variations in dissolved U and PO₄ ^3– with salinity was also found. There are two major mechanisms, desorption from suspended sediments and diffusion from interstitial waters of bottom sediments, that may cause the elevated concentrations of dissolved U and PO₄ ^3– in mid-salinity waters. Mixing experiments indicate that desorption seems more responsible for the elevated dissolved U concentrations, whereas diffusion influences more the enrichment of PO₄ ^3–.     

U-Pb systems and U isotopic composition of the sandstone-hosted paleovalley Dybryn uranium deposit, Vitim uranium district, Russia

The isotopic (U-Pb, ²³⁸U-²³⁵U, ²³⁴U-²³⁸U) and chemical study of whole-rock samples and finegrained fractions of rocks in a vertical section of the terrigenous sequence at the Dybryn uranium deposit in the Khiagda ore field shows that a wide U-Pb isotopic age range (26.9-6.5 Ma) is caused by oxidation and disturbance of the U-Pb isotopic system in combination with protracted uranium ore deposition. The oxidation of rocks resulted in the loss of uranium relative to lead and eventually to an overestimated ²⁰⁶Pb/²³⁸U age at sites with a low U content. The ²³⁸U/²³⁵U ratios in the studied samples are within the range of 137.74–137.88. Samples with a high uranium content are characterized by a decreasing ²³⁸U/²³⁵U ratio with a decrease in ²⁰⁷Pb/²³⁵U and ²⁰⁶Pb/²³⁸U ages. A nonequilibrium ²³⁴U/²³⁸U ratio in most studied samples furnishes evidence for young (<1.5 Ma) transformation of the Miocene uranium ore, which is responsible for uranium migration and its redeposition.     

A study of234U/238U ratios in groundwaters of Taiyuan area,Shanxi Province

Uranium contents and²³⁴U/²³⁸U ratios have been determined on 29 water samples from the Taiyuan area, Shanxi Province. The results show that the same artesian aquifer has similar uranium contents and²³⁴U/²³⁸U activity ratios, and the deeper aquifers have higher A. R. values but lower uranium contents. The A. R. values increase slightly towards groundwater flow in the artesian aquifers dominated by oxidizing ground waters. The Lancun Spring and the famous Jinci Spring belong to two different karst groundwater systems, i.e., the east and west karst groundwater systems. The recharge area of the Lancun Spring should cover the wide limestone outcrops of middle Ordovician in the northeast. The Ordovician fissure-karst ground water to the Jinci Spring is extensively mixed with fissure water in Carboniferous-Jurassic formations and seepage water from the Fenhe River.     

Uranium series disequilibria in the sedimentary uranium deposit at Yeelirrie,Western Australia

The weighted mean values of the ²³⁴U/²³⁸U and the ²³⁰Th/²³⁴U ratios in ore samples collected above the modern water table of the Yeelirrie uranium deposit in Western Australia are 1.38 ± 0.10 and 0.83 ± 0.28, respectively. The relatively larger variability in the latter ratio is evidence for the translocation of uranium subsequent to deposition. Daughter product separation is due to differences in the mobilities of the thorium and uranium species. Factors involved in interpreting the observed ratios, in terms of the dynamics of the accumulation of the deposit, are assessed in terms of an open system model. The observed disequilibria provide a quantitative basis for the evaluation of hypotheses developed from geological and other considerations.     

Spatial and temporal variability of 234U/238U activity ratios in the Shu River,Central Asia

This study presents the temporal and spatial variability of ²³⁴U/²³⁸U activity ratios in the Shu River and provides interpretation to explain the downstream changes of uranium and the ²³⁴U/²³⁸U activity ratios in the study area. The positive linear correlation (R ² = 0.98, p < 0.001) between uranium concentration and specific electrical conductance is consistent with rock weathering and leaching as the major contributor of dissolved uranium in the studied area of the river. The ²³⁴U/²³⁸U activity ratio ranged between ~1.6 in the upper reaches of the river to ~1.15 furthest downstream. Activity ratios at specific sampling points do not show significant seasonal variability.     

Uranium geochemistry on the Amazon shelf: Evidence for uranium release from bottom sediments

In Amazon-shelf waters, as salinity increases to 36.5 × 10⁻³, dissolved uranium activities increase to a maximum of 4.60 dpm 1⁻¹. This value is much higher than the open-ocean value (2.50 dpm 1⁻¹), indicating a source of dissolved uranium to shelf waters in addition to that supplied from open-ocean and riverine waters. Uranium activities are much lower for surface sediments in the Amazon-shelf seabed (mean: 0.69 ±.09 dpm g⁻¹) than for suspended sediments in the Amazon River (1.82 dpm g⁻¹). Data suggest that the loss of particulate uranium from riverine sediments (and the consequent input of dissolved uranium to shelf waters) is probably the result of uranium desorption from the ferric-oxyhydroxide coatings on sediment particles, and/or uranium release by mobilization of the ferric oxyhydroxides. The total flux (i.e., riverine flux plus desorbed-remobilized particulate flux) of dissolved ²³⁸U from the Amazon shelf (about 1.2 × 10¹⁵ dpm yr⁻¹) constitutes about 15% of uranium input to the world ocean, commensurate to the Amazon River's contribution to world river-water discharge (approximately 18%). Measurement of only the riverine flux of dissolved ²³⁸U underestimates, by a factor of about 5, the flux of dissolved²³⁸U from the Amazon shelf to the open ocean.     

Neoproterozoic ice sheets of the Siberian Platform: U-Pb-LA-ICP-MS ages of detrital zircons from the Bol’shoi Patom formation and the geotectonic position of its provenance

The centers of many Neoproterozoic and Phanerozoic glaciations were located on cratons and crystalline shields not necessarily, as some researchers believe, associated with rifts. An example is the Vendian Bol’shoi Patom glacial formation (Lena River, Yakutia). The U-Pb ages of detrital zircons from this formation imply that it was deposited by glaciers located on the pre-Riphean crystalline shields of the Siberian Platform. Glaciation in this region occurred after cessation of rifting and could not be related to the latter. The Bol’shoi Patom Formation is an element of the Middle Siberian glacial horizon that was deposited during the Marino Glaciation and is traceable along the southern periphery of the Siberian Platform from the Aldan Shield to the Baikal and Sayany regions. This indicates that the Marinoan Glaciation in Siberia involved at least the entire southern part of the Siberian Platform. Rifting was not the single, or even a principal, factor responsible for glaciations, although it could accompany and enhance them simultaneously providing space for sedimentation and conditions for preserving glacial deposits from erosion.     

新疆白杨河铍铀矿床萤石Sm-Nd和沥青铀矿U-Pb年代学及其地质意义

白杨河矿床是我国类型独特的一个特大型铍、铀多金属矿床,铍矿物主要确定为羟硅铍石,铀矿物主要发现沥青铀矿和次生的硅钙铀矿以及少量的铌铀矿,伴生矿物主要是萤石。为恢复铀和铍的成矿过程,划分成矿阶段,本次工作通过系统采集钻孔中的萤石样品,进行了Sm-Nd同位素测年研究,获得了三组等时线年龄,分别为291±16Ma、265±33Ma和207±37Ma,代表了成矿前、成矿期和成矿后萤石的形成;采集中心工地、新西工地和九号工地平巷内的沥青铀矿样品,进行了UPb同位素测年研究,获得了~(206)Pb/~(238)U表观年龄237.8±3.3Ma、224±3.1Ma、197.8±2.8Ma、97.8±1.4Ma和30.0±0.4Ma,利用U-Pb表观年龄将铀矿化划分为四个阶段:中三叠世、晚三叠-早侏罗世、晚白垩世和古近纪中期。因此,白杨河矿床具有铍早铀晚的成矿特点,铀成矿经历了四个阶段。     

Behavior and budget of dissolved uranium in the lower reaches of the Yellow (Huanghe) River: Impact of Water–Sediment Regulation Scheme

The Water–Sediment Regulation Scheme (WSRS) is an important water conservancy project in the Yellow River basin, which is usually operated annually from June to July to control water and sediment release from the Xiaolangdi Reservoir in the middle reaches. As a greatly concentrated period of delivering terrigenous materials from the Yellow River to the sea, the WSRS can serve as a natural laboratory to examine the geochemical behavior of elements during their transport along the river. Uranium isotopes (²³⁴U and ²³⁸U) were measured in Yellow River waters at stations Xiaolangdi (located in the middle reaches of the Yellow River) and Lijin (the last hydrologic station near the Yellow River estuary) during the WSRS 2012. Compared with station Xiaolangdi, dissolved uranium concentration at station Lijin was markedly higher, showing a significant impact from the WSRS. Budget calculation for dissolved uranium during the WSRS indicated that two major sources of new added dissolved uranium in the section of the Yellow River between Xiaolangdi and Lijin: suspended particles (46%) and porewater of bottom sediment (45%). The flux of dissolved uranium from the Yellow River to the sea was estimated to be 2.40 × 10⁷ g during the WSRS 2012.     

Uranium isotopes (234U/238U) in rivers of the Yukon Basin (Alaska and Canada) as an aid in identifying water sources, with implications for monitoring hydrologic change in arctic regions

The ability to detect hydrologic variation in large arctic river systems is of major importance in understanding and predicting effects of climate change in high-latitude environments. Monitoring uranium isotopes (²³⁴U and ²³⁸U) in river water of the Yukon River Basin of Alaska and northwestern Canada (2001?C2005) has enhanced the ability to identify water sources to rivers, as well as detect flow changes that have occurred over the 5-year study. Uranium isotopic data for the Yukon River and major tributaries (the Porcupine and Tanana rivers) identify several sources that contribute to river flow, including: deep groundwater, seasonally frozen river-valley alluvium groundwater, and high-elevation glacial melt water. The main-stem Yukon River exhibits patterns of uranium isotopic variation at several locations that reflect input from ice melt and shallow groundwater in the spring, as well as a multi-year pattern of increased variability in timing and relative amount of water supplied from higher elevations within the basin. Results of this study demonstrate both the utility of uranium isotopes in revealing sources of water in large river systems and of incorporating uranium isotope analysis in long-term monitoring of arctic river systems that attempt to assess the effects of climate change.     

Role of Suspended Particulate Matter in Regulating the Behavior of Dissolved Uranium in the Yellow River Estuary

In order to examine the mixing behavior of dissolved uranium (U) in estuaries under different suspended particulate matter (SPM) regimes, three laboratory-based experiments were conducted by mixing seawater with river water containing different concentrations of SPM. Comparing this study with other field and laboratory-based experiments, dissolved U behaved differently depending upon the concentration of SPM. When SPM concentrations are >?0.8 g/L in the Yellow River, desorption/dissolution of U from SPM becomes predominant and dissolved U is enriched relative to the theoretical mixing line. However, when SPM concentrations are <?0.8 g/L, dissolved U behaves conservatively with some extent of removal during estuarine mixing. ²³⁴U/²³⁸U activity ratios were somewhat constant showing no measurable isotopic fractionation during physical mixing and U sorption/desorption to/from particles. Addition of dissolved ²³⁸U desorbed/dissolved from SPM during the annual Yellow River water-sediment regulation scheme (Jun 30th–Jul 14th, 2014) was estimated at 6.4?×?10¹¹ dpm, about 9% of the total riverine flux of dissolved ²³⁸U during that same period. This study represents a contribution to studies of dissolved U in muddy rivers and estuaries throughout the world. Results reported here provide not only a perspective to better estimate U flux from rivers to the ocean but also new insights into better understanding its estuarine mixing behavior and controlling factors.     

A method for determination of the isotopic composition of authigenic uranium in Baikal bottom sediments

A simple, reliable, and high-performance method has been proposed for direct determination of the isotopic composition of authigenic uranium in silica lacustrine sediments. The method is based on studying the kinetics of the selective extraction of authigenic uranium from sediments with weak solutions of ammonium hydrocarbonate followed by the ICP-MS analysis of the nuclides. To estimate the contamination of authigenic uranium by terrigenous one, the contents of ²³²Th and some other clastogenic elements in the extracts were measured simultaneously. The selectivity of extraction of authigenic uranium from the sediments treated with a 1% NH₄HCO₃ solution appeared to be no worse than 99%. The method was used to analyze the isotopic composition of authigenic uranium at several key horizons of a core dated before. The measurements directly prove that the ²³⁴U/²³⁸U values in Baikal water varied depending on climate, which contradicts the previous statements. The measured ²³⁴U/²³⁸U ratios in paleo-Baikal water match the values reconstructed from isotopic data for total uranium in the sediments on the supposition that the U/Th ratio is constant in the terrigenous part of the sediment. Direct experimental determination of total and authigenic nuclides in sediments enhances the potentiality of the method for absolute ²³⁴U-²³⁰Th dating of carbonate-barren lacustrine sediments, including those from Lake Baikal, within the intervals corresponding to the periods of glaciation, where the sediments contain a large fraction of terrigenous component. Given the fractions of terrigenous and authigenic uranium are accurately determined, we have an opportunity to study the variability of the sources of terrigenous matter and to refine the previous model for reconstructing the climate humidity in East Siberia.     

New information on radionuclides concentration in phosphorites originating from Tunisia and Algeria

In this study we investigate the radiological hazard of naturally occurring radioactive material in Tunisian and Algerian phosphorite deposits. Eight samples of phosphorite were collected from the phosphorite mines. The Tunisian and Algerian phosphorites occur in the Late Paleocene and Lower Eocene (Ypresian-Lutetian) in age (Béji Sassi 1984 and Zaïer 1999). Activity concentrations in all the samples were measured by alpha spectrometry and gamma spectrometry. Alpha spectrometry analyses show that the specific activity values of ²³⁸U, ²³⁴U and ²³⁵U in the samples of Tunisian phosphorite were 327?±?7 (321–327), 326?±?6 (325–331) and 14.50?±?0.72 (13.90–15.57) Bq kg^?1, respectively. Specific activity measured by gamma spectrometry in the samples of the Tunisian and Algerian phosphorite shows a small difference. Specific activity levels of ⁴⁰K, ²²⁶Ra, ²³²Th, ²³⁵U and ²³⁸U in the phosphorite samples from Tunisia were, respectively, 71.10?±?3.80, 391.54?±?9.39, 60.38?±?3.74, 12.72?±?0.54 and 527.42?±?49.57 Bq kg^?1 and Algeria were 15.72?±?1.73, 989.65?±?12.52, 12.08?±?1.20, 47.50?±?1.52 and 1,148.78?±?7.30 Bq kg^?1, respectively. The measured value of specific activity of ²³²Th and ⁴⁰K in the Tunisian phosphorite samples is relatively higher than that found in the samples of Algerian phosphorite. The measured activity of uranium (²³⁸U) in the Tunisian phosphorite (527?±?49) Bq kg^?1 is lower than in Algerian phosphorite. The measured activity of ²³⁸U in the Tunisian phosphorite samples was (527–1,315?±?65) ²³⁸U Bq kg^?1 which is higher than its maximum background value of 110 Bq kg^?1 in soils of the various countries of the world (Tufail et al. Radiat Meas 41:443–451, 2006). Different geological origins of phosphorites deposits are the main reason for the large spread in worldwide specific activities. The obtained results of uranium concentrations in phosphorites of different types (Algerian and Tunisian) demonstrate that the uranium concentrations are mainly governed by the phosphatic material. The present study reveals that phosphorite deposits contain natural radioactivity higher than background level.     

Processes controlling 234U and 238U isotope fractionation and helium in the groundwater of the St. Lawrence Lowlands,Quebec: The potential role of natural rock fracturing

The goal of this study is to explain the origin of ²³⁴U–²³⁸U fractionation in groundwater from sedimentary aquifers of the St. Lawrence Lowlands (Quebec, Canada), and its relationship with ³He/⁴He ratios, to gain insight regarding the evolution of groundwater in the region. (²³⁴U/²³⁸U) activity ratios, or (²³⁴U/²³⁸U)_act, were measured in 23 groundwater samples from shallow Quaternary unconsolidated sediments and from the deeper fractured regional aquifer of the Becancour River watershed. The lowest (²³⁴U/²³⁸U)_act, 1.14 ± 0.01, was measured in Ca–HCO₃-type freshwater from the Quaternary Shallower Aquifer, where bulk dissolution of the carbonate allows U to migrate into water with little ²³⁴U–²³⁸U isotopic fractionation. The (²³⁴U/²³⁸U)_act increases to 6.07 ± 0.14 in Na–HCO₃–Cl-type groundwater. Preferential migration of ²³⁴U into water by α-recoil is the underlying process responsible for this isotopic fractionation. An inverse relationship between (²³⁴U/²³⁸U)_act and ³He/⁴He ratios has been observed. This relationship reflects the mixing of newly recharged water, with (²³⁴U/²³⁸U)_act close to the secular equilibrium and containing atmospheric/tritiogenic helium, and mildly-mineralized older water (¹⁴C ages of 6.6 kyrs), with (²³⁴U/²³⁸U)_act of ≥6.07 and large amounts of radiogenic ⁴He, in excess of the steady-state amount produced in situ. The simultaneous fractionation of (²³⁴U/²³⁸U)_act and the addition of excess ⁴He could be locally controlled by stress-induced rock fracturing. This process increases the surface area of the aquifer matrix exposed to pore water, from which produced ⁴He and ²³⁴U can be released by α-recoil and diffusion. This process would also facilitate the release of radiogenic helium at rates greater than those supported by steady-state U–Th production in the rock. Consequently, sources internal to the aquifers could cause the radiogenic ⁴He excesses measured in groundwater.